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大气中丙烷光氧化臭氧生成活性的烟雾箱模拟
摘要点击 1569  全文点击 1315  投稿时间:2011-10-21  修订日期:2012-01-12
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中文关键词  烟雾箱  丙烷  光化学反应  相对湿度  臭氧  丙酮
英文关键词  smog chamber  propane  photochemical reaction  relative humidity  ozone  acetone
作者单位E-mail
黄丽华 广西大学环境学院, 南宁 530004
中国科学院大气物理研究所大气边界层物理和大气化学国家重点实验室, 北京 100029 
hlh@smoglab.org 
莫创荣 广西大学环境学院, 南宁 530004  
徐永福 中国科学院大气物理研究所大气边界层物理和大气化学国家重点实验室, 北京 100029 xyf@mail.iap.ac.cn 
贾龙 中国科学院大气物理研究所大气边界层物理和大气化学国家重点实验室, 北京 100029  
中文摘要
      利用自制光化学烟雾箱模拟了丙烷和NOx大气光化学反应,研究了相对湿度以及丙烷与NOx初始浓度比值对臭氧生成的影响.实验表明,臭氧最大值及丙烷的臭氧生成活性最大值(IRmax)都随相对湿度的增大而减小.低相对湿度时,臭氧最大值大约出现在反应的22 h,IRmax变化范围为0.0231~0.0391; 而高相对湿度时,臭氧最大值大约出现在反应的16 h,IRmax变化范围为0.0172~0.0320.在反应的20 h内,前12 h内相对湿度对丙酮的生成量影响不大,12 h后低相对湿度时丙酮生成量更大.在实验的4~20 h内,相对湿度为17%时,丙酮浓度为153×10-9~364×10-9; 而相对湿度为62%时,丙酮浓度为167×10-9~302×10-9.臭氧最大值随着丙烷与NOx初始浓度比值增加而减少,在低相对湿度时线性负相关性更好.另外,还利用了MCM丙烷子机制对反应进行了数值模拟,并与实验结果进行比较,发现两者还存在较大的偏差.
英文摘要
      Atmospheric photochemical reactions of propane and NOx were simulated with a self-made smog chamber. The effects of relative humidity (RH) and [C3H8]0/[NOx]0 ratio on ozone formation were studied. The results showed that both the maximum ozone concentration and the maximum value of incremental reactivity (IRmax) of propane decreased linearly with increasing RH. Under lower RH conditions, the occurrence time of peak ozone concentration was about 22 h after the beginning of reaction, and IRmax varied from 0.0231 to 0.0391, while under higher RH conditions the occurrence time of peak ozone concentration was 16 h, and IRmax ranged from 0.0172 to 0.0320. During the 20 h of reaction, within the first 12 h RH did not significantly affect the yield of acetone, whereas after 12 h the lower RH condition could lead to relatively greater amount of acetone. During the first 4-20 h of experiments, acetone concentrations ranged from 153×10-9 to 364×10-9 at 17% RH and from 167×10-9 to 302×10-9 at 62% RH, respectively. Maximum ozone concentrations decreased with increasing [C3H8]0/[NOx]0 ratio and a better negative linear relationship between them was obtained under the lower RH conditions. The smog chamber data and the results from simulation of the C3H8-NOx reactions using the sub-mechanism of MCM were compared, and a significant deviation was found between these two results.

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